{"title":"高活性、高耐久性甲醇化产物气体氢还原乙醇脱水加氢催化剂的研制","authors":"Shimpei Norioka, Tomoki Uchiyama, Hirofumi Ohtsuka, Yoshiharu Uchimoto","doi":"10.1007/s10562-025-05147-w","DOIUrl":null,"url":null,"abstract":"<div><p>Methanation, the production of methane from CO<sub>2</sub> and hydrogen, is attracting increased attention as a measure to reduce carbon dioxide emissions from fossil fuel combustion. To use methanation product gas as city gas, reducing the amount of hydrogen in the methanation product gas remains a key challenge. To achieve this, a catalytic system has been proposed that uses ethanol, a widely used biofuel, and the hydrogen in methanation product gas to drive the ethanol dehydration–hydrogenation reaction. In this study, we found that the Pd/HSiW/SiO<sub>2</sub> catalyst initially exhibited high activity but gradually lost its activity due to reactions with water vapor contained in the reaction gas, as revealed by various measurements. On the other hand, Pd/WO<sub>3</sub>/ZrO<sub>2</sub>, which initially had relatively low activity and low selectivity, did not degrade after 150 h of continuous activity measurement, and the activity and selectivity of the reaction increased during the test. The increase in the activity of WO<sub>3</sub>/ZrO<sub>2</sub> after hydrogen pretreatment was investigated by NH<sub>3</sub>-TPD, and it was concluded that this increase was due to an increase in the solid acid strength caused by hydrogen in the gas. These results indicate that Pd/WO<sub>3</sub>/ZrO<sub>2</sub> is both highly active and highly durable for dehydration–hydrogenation of ethanol and is suitable for practical applications.</p><h3>Graphical Abstract</h3><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":"155 9","pages":""},"PeriodicalIF":2.3000,"publicationDate":"2025-08-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Development of an Ethanol Dehydration–Hydrogenation Catalyst for Reducing Hydrogen Content in Methanation Product Gas with High Activity and High Durability\",\"authors\":\"Shimpei Norioka, Tomoki Uchiyama, Hirofumi Ohtsuka, Yoshiharu Uchimoto\",\"doi\":\"10.1007/s10562-025-05147-w\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Methanation, the production of methane from CO<sub>2</sub> and hydrogen, is attracting increased attention as a measure to reduce carbon dioxide emissions from fossil fuel combustion. To use methanation product gas as city gas, reducing the amount of hydrogen in the methanation product gas remains a key challenge. To achieve this, a catalytic system has been proposed that uses ethanol, a widely used biofuel, and the hydrogen in methanation product gas to drive the ethanol dehydration–hydrogenation reaction. In this study, we found that the Pd/HSiW/SiO<sub>2</sub> catalyst initially exhibited high activity but gradually lost its activity due to reactions with water vapor contained in the reaction gas, as revealed by various measurements. On the other hand, Pd/WO<sub>3</sub>/ZrO<sub>2</sub>, which initially had relatively low activity and low selectivity, did not degrade after 150 h of continuous activity measurement, and the activity and selectivity of the reaction increased during the test. The increase in the activity of WO<sub>3</sub>/ZrO<sub>2</sub> after hydrogen pretreatment was investigated by NH<sub>3</sub>-TPD, and it was concluded that this increase was due to an increase in the solid acid strength caused by hydrogen in the gas. These results indicate that Pd/WO<sub>3</sub>/ZrO<sub>2</sub> is both highly active and highly durable for dehydration–hydrogenation of ethanol and is suitable for practical applications.</p><h3>Graphical Abstract</h3><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>\",\"PeriodicalId\":508,\"journal\":{\"name\":\"Catalysis Letters\",\"volume\":\"155 9\",\"pages\":\"\"},\"PeriodicalIF\":2.3000,\"publicationDate\":\"2025-08-18\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Catalysis Letters\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://link.springer.com/article/10.1007/s10562-025-05147-w\",\"RegionNum\":4,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q3\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Catalysis Letters","FirstCategoryId":"92","ListUrlMain":"https://link.springer.com/article/10.1007/s10562-025-05147-w","RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Development of an Ethanol Dehydration–Hydrogenation Catalyst for Reducing Hydrogen Content in Methanation Product Gas with High Activity and High Durability
Methanation, the production of methane from CO2 and hydrogen, is attracting increased attention as a measure to reduce carbon dioxide emissions from fossil fuel combustion. To use methanation product gas as city gas, reducing the amount of hydrogen in the methanation product gas remains a key challenge. To achieve this, a catalytic system has been proposed that uses ethanol, a widely used biofuel, and the hydrogen in methanation product gas to drive the ethanol dehydration–hydrogenation reaction. In this study, we found that the Pd/HSiW/SiO2 catalyst initially exhibited high activity but gradually lost its activity due to reactions with water vapor contained in the reaction gas, as revealed by various measurements. On the other hand, Pd/WO3/ZrO2, which initially had relatively low activity and low selectivity, did not degrade after 150 h of continuous activity measurement, and the activity and selectivity of the reaction increased during the test. The increase in the activity of WO3/ZrO2 after hydrogen pretreatment was investigated by NH3-TPD, and it was concluded that this increase was due to an increase in the solid acid strength caused by hydrogen in the gas. These results indicate that Pd/WO3/ZrO2 is both highly active and highly durable for dehydration–hydrogenation of ethanol and is suitable for practical applications.
期刊介绍：
Catalysis Letters aim is the rapid publication of outstanding and high-impact original research articles in catalysis. The scope of the journal covers a broad range of topics in all fields of both applied and theoretical catalysis, including heterogeneous, homogeneous and biocatalysis.
The high-quality original research articles published in Catalysis Letters are subject to rigorous peer review. Accepted papers are published online first and subsequently in print issues. All contributions must include a graphical abstract. Manuscripts should be written in English and the responsibility lies with the authors to ensure that they are grammatically and linguistically correct. Authors for whom English is not the working language are encouraged to consider using a professional language-editing service before submitting their manuscripts.
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